Electrocatalytic CO2 hydrogenation to C2+ alcohols catalysed by Pr–Cu oxide heterointerfaces
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Mechanisms of electrochemical hydrogenation of aromatic compound mixtures over a bimetallic PtRu catalyst
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Enantioselective C–H annulations enabled by either nickel- or cobalt-electrocatalysed C–H activation for catalyst-controlled chemodivergence
Enantioselective electrocatalysis shows unique potential for the sustainable assembly of enantiomerically enriched molecules. This approach allows electro-oxidative C–H activation to be performed paired to the hydrogen evolution reaction. Recent progress has featured scarce transition metals with limited availability. Here we reveal that the earth-abundant 3d transition metals nickel and cobalt exhibit distinctive performance for enantioselective electrocatalysis with chemodivergent reactivity patterns. Enantioselective desymmetrizations of strained bicyclic alkenes were achieved through C–H annulations. A data-driven optimization of chiral N,O-bidentate salicyloxazoline-type ligands was crucial for enhancing enantioselectivity in nickel electrocatalysis. Notably, in the transition state of the enantio-determining step, secondary weak attractive π–π and CH–π interactions were identified, reflecting the informed adaptations in the ligand design. Detailed mechanistic investigations by experimental and computational studies revealed for the nickel electrocatalysis a C–N bond-forming reductive elimination from nickel(III) and for the cobalt electrocatalysis a C–C bond-forming nucleophilic addition from cobalt(III) as the product-determining steps.
Electrocatalytic mechanism for overall water splitting to produce sustainable hydrogen by 2D Janus MoSH monolayer
In the present work, we investigates the potential of two dimensional (2D) Janus MoSH monolayer as an electrocatalyst for overall water splitting using first-principles calculations. Our results shows that 2D Janus MoSH monolayer exhibits excellent structural stability and electronic properties, which are essential for efficient electrocatalysis. We find that the charge transfer mechanism between Mo and S atoms plays a crucial role in the electrocatalytic activity of 2D Janus MoSH monolayer. Due to the asymmetric structure of MoSH monolayer, it has intrinsic electric field with dipole moment of 0.24 D. Moreover, we demonstrate that 2D Janus MoSH monolayer exhibits high catalytic activity for both hydrogen evolution reaction (HER) with overpotential 0.04 V and oxygen evolution reaction (OER) with overpotential 0.11 V, making it a promising candidate for overall water splitting. Our findings have significant implications for the design and optimization of 2D monolayered materials for renewable energy production. By providing insights into the underlying mechanisms of HER and OER on 2D Janus MoSH monolayer, our study paves the way for the development of efficient and sustainable electrocatalysts for water splitting. We hope that current work will be helpful in understanding the electrocatalytic mechanism of 2D Janus MoSH monolayer and its potential applications in renewable energy production.
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